First Principles Calculation of the Thermal Volume Expansion Coefficient of Tetragonal Zircon Dioxide

Abstract

We present a general method to calculate thermodynamical properties of crystalline materials from first principles based on density functional theory (DFT). In order to introduce temperature effects we calculate the phonon dispersion for different volumes which allows to include their entropic effects in the Helmholtz free energy. As an example we focus on the calculation of the thermal volume expansion coefficient of tetragonal ZrO2.

Calculation of the anisotropic coefficients of thermal expansion: A first-principles approach

“…While experimental measurements of the coefficient of thermal expansion (CTE) can be done using a number of experimental techniques 1-5 , most theoretical tools available for predicting the CTE are limited to the quasiharmonic approximation (QHA) or the Debye-Gruneisen approximation. There are a few programs 6,7 and several models [8][9][10][11][12][13][14][15][16][17] available for scientists to calculate the CTE, and its associated thermal properties, from firstprinciples calculations. These currently available methods principally rely on the QHA.…”

Oxide‐Based Solid‐State Batteries: A Perspective on Composite Cathode Architecture

“…In computational modeling, there exist methodologies to estimate the CTE of bulk materials using DFT based atomistic simulation techniques. [ 84 ] The CTE for LCO‐type CAMs, as predicted by atomistic simulations, demonstrates a strong dependence on the temperature of operation as well as the amount of Li present within the layered CAM phase. [ 85 ] However, such low length scale approaches have not yet been adopted for estimating the CTE for LLZO SEs.…”